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Issue 4, 2013
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Electrochemical reactivities of pyridinium in solution: consequences for CO2 reduction mechanisms

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Abstract

One of the most promising CO2 reduction processes presently known suffers from a lack of fundamental understanding of its reaction mechanism. Using first principles quantum chemistry, we report thermodynamical energies of various pyridine-derived intermediates as well as barrier heights for key homogeneous reaction mechanisms. From this work, we predict that the actual form of the co-catalyst involved in pyridinium-based CO2 reduction is not the long-proposed pyridinyl radical in solution, but is more probably a surface-bound dihydropyridine species.

Graphical abstract: Electrochemical reactivities of pyridinium in solution: consequences for CO2 reduction mechanisms

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Publication details

The article was received on 21 Dec 2012, accepted on 11 Feb 2013 and first published on 14 Feb 2013


Article type: Edge Article
DOI: 10.1039/C3SC22296A
Citation: Chem. Sci., 2013,4, 1490-1496
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    Electrochemical reactivities of pyridinium in solution: consequences for CO2 reduction mechanisms

    J. A. Keith and E. A. Carter, Chem. Sci., 2013, 4, 1490
    DOI: 10.1039/C3SC22296A

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